Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy

Li Zhang, Xiaoju Yang, Qing Yuan, Zhiming Wei, Jie Ding, Tianshu Chu, Chao Rong, Qiao Zhang, Zhenkun Ye, Fu-Zhen Xuan, Yueming Zhai, Bowei Zhang () and Xuan Yang ()
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Li Zhang: Huazhong University of Science and Technology
Xiaoju Yang: Huazhong University of Science and Technology
Qing Yuan: Huazhong University of Science and Technology
Zhiming Wei: Wuhan University
Jie Ding: Wuhan University
Tianshu Chu: East China University of Science and Technology
Chao Rong: East China University of Science and Technology
Qiao Zhang: Wuhan University
Zhenkun Ye: Huazhong University of Science and Technology
Fu-Zhen Xuan: East China University of Science and Technology
Yueming Zhai: Wuhan University
Bowei Zhang: East China University of Science and Technology
Xuan Yang: Huazhong University of Science and Technology

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Understanding the structure-stability relationship of catalysts is imperative for the development of high-performance electrocatalytic devices. Herein, we utilize operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to quantitatively monitor the evolution of Cu single-atom catalysts (SACs) during the electrochemical reduction of CO2 (CO2RR). Cu SACs are converted into 2-nm Cu nanoparticles through a reconstruction process during CO2RR. The evolution rate of Cu SACs is highly dependent on the substrates of the catalysts due to the coordination difference. Density functional theory calculations demonstrate that the stability of Cu SACs is highly dependent on their formation energy, which can be manipulated by controlling the affinity between Cu sites and substrates. This work highlights the use of operando ATR-SEIRAS to achieve mechanistic understanding of structure-stability relationship for long-term applications.

Date: 2023
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DOI: 10.1038/s41467-023-44078-1

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